Process of producing chemical



Aug. 6,1940. w. w. ODELL PROCESS OF PRODUCING CHEMICAL REACTIONSOriginal Filed Dec. 1'7. 1929 2 Sheets-Sheet 1 2 l 3 p n V 3 6 a r. i 5b b 7 n L i m wmt Phil! 1\\1\\ 7 1 1 2 W. W. ODELL PROCESS OF PRODUCINGCHEMICAL REACTIONS Original Filed Dec. 17. 1929 2 Sheets-Sheet 2 ReiauedAug. 6, 1940 UNITED STATES PATENT OFFICE raoonss or raonucmc. CHEMICALnEAo'rroNs William W. Odell, Lutherville, Md.

12' Claims.

This invention relates to the process of treating crushed solids,fluids, including gases, or both, and causing physical, chemical, orboth physical and chemical changes to occur in said solids. fluids or inboth solids and fluids. Essentially it is a process wherein crushed,conflned solids are fluidized by suspension in a fluid stream and inthis condition are treated with a. fluid of which the nature,temperature, pressure, humidity and other constants as well as velocityare controlled.

The true scope of my invention is made more apparent by the numerousobjects, some of which are listed as follows:

(1) Carbonize coal by passing a fluid at a suitable, predeterminedtemperature through a fluidized mass of suitably crushed coal.

(2) Remove moisture or other volatile matter from fluidized solids.

(3) Cause chemical change in the composition of a fluid by passing itthrough a fluidized mass of solids, for example, production of carbonblack from natural gas.

(4) Control the rate of heating and therefore the nature and yield ofby-products in the carbonization of coal.

(5) Control temperature of a mass of solids used-in treating gases, ormore broadly, in treating fluids.

Other objects will become apparent by disclosures made in a subsequentportion of the specifications; likewise the fleld of applicability of myinvention will become obvious.

Briefly, my process consists in passing a particular fluid stream havingpredetermined composition, temperature, velocity, humidity and density,under controlled pressure, through a mass of crushed solids or theequivalent, causing the mass of solids to become fluidized, that is, tobehave like a liquid, and causing physical, chemical or both physicaland chemical changes to occur in the solids, or fluid, or in both solidsand fluid.

Considering as an example, the carbonization of coal, it is commonknowledge that because of heat transfer. difficulties the commercialdevelopment of low-temperature carbonization processes have thus farbeen frustrated. Dependence upon the passage of heat through refractorywalls with a low temperature-gradient has made necessary the expenditureof prohibitive sums of money for carbonization apparatus. Applying myprocess, I can, so far as I am aware, accomplish the result sought at alower cost and greater efliclency than is obtaine in other processes,and with absolute temper ture control, by passing a heated fluidupwardly through a mass of crushed coal contained in a suitable chamber,at such a velocity that the particles or pieces of the coal are inconstant motion, the mass assuming in the fluidized condition theproperties of a boiling liquid. 5 If the particles are all uniform insize, M inch in average diameter, the tendency is for the hottest onesto rise and the colder and the heavier particles to go to the bottom.The temperature of the fluid may be increased with time to any desiredmaximum, and the coal particles will thus not become overheated. Thefluid used in this example may be a vapor or gas (combustible, inert, oran oxygen containing gas or mixtures), steam, or other suitable fluid;some of the evolved products may be recirculated as a means ofcontrolling the temperature and the atmosphere in the chamber.

In this example the solids are changed physically and chemically and theprimary or original fluid may or may not be changed, according to thetemperature reached and the composition of said fluid. Thus, if air. isthe fluid medium, some of its oxygen is consumed by the oxidation of thecoal; when steam is the fluid medium, it reacts at elevated temperaturesby the well known water gas reaction.

Another example is the passage of mixtures of hydrogen and carbonmonoxide through a mass of fluidized particles of iron-copper catalyst(or other suitable catalyst) at a temperature of about 300 C.200 to 450C. Here the fluidizing medium comprises the mixed C0 and H: which reactwith one another yielding hydrocarbons or other compounds and thechemical nature of the solids is substantially unchanged. The reactionbeing exothermic, there is a tendency for the temperature to rise in themass. Increasing the velocity of the fluid decreases the time and theintimacy of its contact with the catalyst and therefore decreases theamount of reaction and the temperature rise. In this manner, or bycirculating the fluidized catalyst through a cooling system, thetemperature of the catalyst is readily controlled. The gasesrecirculated may flrst be cooled. 45

By passing natural gas or other gaseous hydrocarbon or vaporizedhydrocarbon upwardly through a. mass of fluidized, heated carbonaceousmaterial or other catalyst, I am able to produce carbon black underoptimum conditions, since the temperature and concentration of gases andtime of contact can be accurately controlled within definite limits aswell as the temperature of the catalyst mass. When anthracite coal, cokeor other carbonaceous material capable of withstanding high temperatureand capable of being fluidizedhusedasthecatalysbairorotheroxidising'agent may be used as a means of heating the fluidised solids.This air or oxidizing agent may be introduced along with the gases to betreated or the operation may be intermittent.

Having briefly described the pertinent features peculiar to theoperation of my process. a more detailed description is given in thefollowing with particular reference to the drawings. This process lendsitself to use in various and numerous types of apparatus but it is theinventors aim to show only a few of these, largely diagrammatically, notconfining himself to the types shown. in the practice oi his invention.

Hg. 1 is a diagrammatic elevation showing one form of apparatus forcarrying out my process. connected with a booster and condensing andscrubbing apparatus; a portion of the reaction chamber wall is cut awayto show the interior.

Fig. 2-is a tie elevation of a modiflcation oi the reaction chamberadapted to the circulation of the fluidised solids. A portion of theshells are cut away to show the interior in section.

In Figure l, numeral I designates the reaction chamber containing a massof fluidized solids 2 and having an inlet for solids I connected withthe hopper l. A mixing mechanism is shown at I which is operated bymotor II. The discharge control valve II regulates the discharge ofsolids into receiver I2. Another discharge valve is shown at I. A grate,perforated plate, porous plate or equivalent is shown at I. The fluidsfrom I discharge through outlet I3 connecting with a dust catcher I4.condenser or heat exchanger I5, scrubber or separator I! and outletvalve is. A means for propelling the fluidizing medium the fluid-4sshown at H. Other valves in the system are shown at II to 43 inclusive.Thus a means for recirculating a portion-or all of the fluid consists inccntrolling valves II, 20, ll, 25, and 28, valves 2!, I, I and II beingclosed. By closing valves ll, 21, II and I0, and opening valves I8, 2.,22, I! and II, the sensible heat of the outgoing fluid is partlyretrieved from the condenser; valve 28 may be closed or partly closed,according to the relative amount of recirculation desired. Similarly,valves ll, 21, II, I, II or combinations of them may be opened or partlyp ned to produce a desired eflect with respect to temperature controland regulation of the composition of the fluid entering chamber I.Vapors. particularly gases other than air, may be admitted to I throughvalves Ii and SI.

InI'igureZthesamesystemofnumberingis used as in Figure 1. IA is a valvesimilar to i, and IA is a mass of subdivided solids which may or may notbe fluidised. The mass of solids 2 is in a fluidised state duringoperation the same as with the awaratus shown in Figure 1.

The dust catcher I4 has means for preventing particles entrained in thegas strain from chamber I from carrying over into II; the means arediagrammatically shown in Figure l by bailles II and ll.

Considering the process with particular reference to the carbonizationof carbonaceous substances such as coal, lignite and the like, theoperation referring to Figure l is as follows: Assuming that thesubstance to be treated is a non-coking coal or lignite, and that all ofthe enumerated valves are closed except 3| which supplies a small pilotlight, on the premix principle, that is, with gas mixed with suflicientair for its combustion; open valve l and admit the suitably crushedcoal, ,i-inch or larger or smaller average size and preferably uniformlysized, into reaction chamber I to a depth of about 2 feet. Now closevalve 5, open valves IO, IO, 32 and 2B and start blower II. Mixingdevice I may be lowered until it is in a position to mix the coal,having previously started motor II. The mechanical means of raising orlowering I are not detailed because patentable novelty is. not claimedthereon and because of a desire to eliminate unnecessary details. Ahollow outer shaft with a counter weighted inner shaftsupporting themixing blades is one means of accomplishing the purpose. The mixerprevents holes forming in the bed and helps in starting to produce afluidized mass of coal.

Air is passed through 2, I1, and tuyere 3 and through the fluidizedmass. Air is the fluidizing agent at this step or stage in the processin this example. A fire is now kindled in the mass. If the air used ishot, ignition will be spontaneous.

,Otherwise it is preferable to initiate it. This may be done by openingvalve 31 allowing ignited, premixed combustible gas and air into chamberI beneath the porous bottom I. A proper pressure balance is maintainedin the air and gas systems, and the coal particles soon become hot andignited. Valve 31 is now closed.

The chamber now may be viewed as a furnace in which the fluidized massbehaves like a boiling liquid, the particles of solid fuel being inmotion in suspension. Combustion and the rate of combustion are nowcontrolled by limiting the amount of air introduced and by introducingother fluids such as steam, or hot gases-combustible or noncombustible.The latter operations may be performed by controlling and regulatingvalves 2|, I9, II, II, 25, 34, 35, 36, 3! and II. Since it is desirableto maintain the solids in a fluidized state, the velocity and flow offluid should be maintained through tuyeres I. More coal is admittedperiodically or continuously through valve 5. Mixer 9 is raised as theaddition of fuel raises the level of the fluidized mass or it may beraised entirely out of the mass; it is usually not required when themass is once properly fluidized unless the coal is strongly coking andis introduced into chamber I at too fast a rate.

Valve 26 is a primary air control-valve. When preheated air is used itmay be drawn in through 1|, condenser l5, valves 22 and II to propelleror booster II. Gas may be preheated in the same manner. Both gas and airmay be preheated'in chamber is in a similar manner by drawing the air inthrough valve II and the gas through 2.. Other possible combinations areevidenced by Figure 1. Steam is introduced into I through valve 3|.

Although fundamentally this method of carbonizing coal comprises thepassage of hot gases upwardly through a bed of fluidized coal,nevertheless, the steps from this point on are some-,

what optional depending upon the result sought, For example, when amaximum yield of condensable by-products is desired, steam can beadvantageously used as a heating fluid, either along with some air orgas, alone, or with the tion from [m ll, heat exchanger ll, separator Itand out through It and it. When recirculaof a portion of the gas issought, valve II is partly closed. valve II partly opened, and valves IIand II are opened. When it is desired to use preheated recirculated gas.valve 24 is closed. valves ll, 22, II and II are open. when preheatedair is desired as a fluid, valves 23, I l. 2. and 21 are closed andvalves II, 22 and 25 are The process is made continuous by merelywithdrawing some of the solid product of carbonization, coke or char inthis example, through valve and charging fuel to be treated throughvalve I. After closing valve 5, the char may be cooled by passing acooling fluid through valve ll, chamber l2 and outlet ll andsubsequently removed through valve 2..

Since the temperature throughout the fluidized mass tends to equalizeitself-tends to uniformity-because the cooler particles tend to sinkinto the combustion none and the hot particles tend to rise, athermocouple and pyrometer may be used to indicate the state and degreeof carboniastion, the former being located in the fluidized mass. Forsimplicity the pyrometer or thermocouple is not shown in the iiguru.

It is possible, in the arrangement shown in Figure 1 to use as a fluid,air, steam, gas, vapor or other fluid or mixtures of the fluids, andthey may be hot or cold or vary with time. In expelling certain volatilematter from coal or from other solids, vaporiaed liquids such as benaol.phenol, toluol, or other hydrocarbons or hydrocarbon compounds may beused advantageously. The choice of the hydrocarbon or the like maydepend upon and vary with the temperature and solvent action desired.

I flnd that, when certain acids or oxidizing agents are used in treatingthe fluidized coal, the swelling properties of coal are eliminated and aproduct is obtained at low temperature which can be mixed withbituminous coal, briquetted without or with a binder and subsequentlycarbonized. the carbonized. briquet being denser than ordinary coke. Iflnd that 80s, H2804, Ch, HCl. HNOa, oxychlorldes and other materialsaid in bringing about this result. They may be used without air, aloneor in mixtures. The process upon which I seek Letters Patent includesthe passage of such'substances through a bed of fluidised solids.

Figure 1 reveals means for causing a fluid to fluidise a mass ofsubdivided solids, means for passing a predetermined fluid or mixture offluids through said fluidized mass, means for controlling thetemperature of said mass, means for changing at will the composition andnature of the fluid and fluidizing medium. means for in troducing solidsinto the fluidized mass, and means for discharging fluids and solidsfrom the reaction chamber. In the carbonization or dis tillation of coalor shale, chamber l5, designated as a heat exchanger, may be a condenserand chamber It a scrubber.

Another example of the operation of my .process is the production ofcarbon black from hydrocarbons. In this process difliculty has beenencountered in the avoidance of the formation of "lamp .black, acarbonaceous substance brownblack to gray-black in color comprisingparticles usually much larger than those of the true carbon-black. Thesecret lies in the accurate control of temperatures during thedecompositioncracking-of the hydrocarbon vapors and con trolofthetime(duration) cftbeirexposureto the action oi heat. when these vapors arecaused to contact a stationary mass of checkered or loosely packed,intermittently heated refractory material confined in an ordinarychamber, the surface temperature of the refractory materlals decreasesso rapidly that lamp-black is usually formed instead of carbon black.when the vapors are passed through a similarly heatedbedofsolidi'ueiaratherlowgradeofcarbonblack is formed but it is notreadily recovered; much of it adheres to the surface of the fuel orremains in the interstices and is subsequently consumed (burned) duringthe heating stage of operation, namely during an air-blasting period.when the vapors or gaseous hydrocarbons are passed through a fluidisedmass of highly heated particles or pieces of solid substance-catalystagood quality of carbon-black and a high yield of it are obtained.Fortunately coke and certain other combustible substances catalyze thereactions and thus it is a simple matter to control the temperature ofthe surface of the catalyst. Iron, iron oxide and other substances alsofunction as catalysts in the production of carbonblack. Some air orother oxidizing agent can be used along with (simultaneously with) theintroduction of the hydrocarbon vapors or alternated with the lattervapors. The concentration and temperature of gas and catalyst canreadily be controlled by means already described, includingrecirculation of gases and by combustion of gases in contact with thefluidised mass.

Whenacatalystisused.otherthanacombustible substance, in chamber I, thetemperature may be maintained uniform either by recirculating thecatalyst or by using air or other;

fluid of controlled temperature. .Cold air can bedrawninthroughltand IIand warmair through 2|, ll, 2!, II, and I]. It is desirable to maintaina quite deflnite temperaturein the fluidised mass during'the cracking ofhydrocarbons and the optimum temperatures are not identical for allgases andvapors. but is deter- 'minsd by experiment. All of the detailsof operation are not presented here since the claims are not conflned tothis-operation but rather to theprouas broadly. However. it should benoted that in thisinstance-the use of mixing device 9 is not necessary.particularly after the solids are fluidised.

The average sins of the solids-coke or the equivalent-should be small,preferably less than inch; the 5 inch average diameter is highlysatisfactory. The solids are added to thereactionchamberthroughvalveiasnecessary and are withdrawn from time totime to avoid the accumulation of clinker. With petroleum coke or highgrade anthracite coal. less attention is required because of less ashaccumulation.

in the continuous production of carbon-blackfrom hydrocarbons such asmethane or natural gas, hydrogen is evolved as a decomposition product.the reaction being typified or repre sented by the equation as follows:

when the hydrogen is recirculated and air is simultaneously introducedinto the reaction chamber (shown at I in Fig. i)- an appreciable amountof the hydrogen is burned. forming water vapor. This seems to be helpfulin producing a high grade carbon-black besides being the means wherebythe necessary heat is supplied. In otherwords,theprcsenceofHs0vaporappearstoenertabeneflcialeflectuponthequalityofblack produced. The consumption ofthe solid carbon comprisingthefluidisedmassisverylowwhentheheatenergytotheprocessissupplied by the hydrogen. Under theseconditions small amoimts of by-products are obtained including bensoland varying in composition and quantity with the temperature employed inthe fluidised mass and the nature of the hydrocarbonusedasrawmaterials.Thecarbonblack is separated from the gases and other products by wellknown means.

Oilshalecanbetreatedbythisprocessand high yieldsoioiiobtained.Itispreferablein thisinstancetousesteamasafluidorasaiiuidcomponent andto burn some of the recirculatedgasesasameansoiheatingtheshalebycontact. Excessive combustion and theuse of an excessive amount of air is avoided to prevent the burning ofappreciable amounts of the shale oil. It should be noted that means areprovided whereby the heating gas may be admitted with just suflicientair for its combustion, hence in the use of recirculated gases, vaporsof chosen hydrocarbons, steam, mixtures, or the like, excessivecombustion need not take place in the reaction chamber.

Combustion is one means of control of temperature in my process and Ipromote combustion in a manner adapted to apply the evolved heat atlocations where heat is required without overheating portions of thefluidized mass. It will be noted that by merely operating valvescombustion may be an alternate cycle or a continuous cycle with theintroduction 0! fluids into the fluidized mass; and that some or all ofthe fluirflzed solids may be drawn from the reaction chamber at will,even during operation.

I do not limit myself to the use of the particular apparatus shown inthe flgures. in'the practice of my process. Various other types oiapparatus can readily be conceived which would also function. Forexample. the solids may be introduced into the reaction chamber atsubstantially the bottom instead of at the top thereof. and likewisethesolids may be periodically discharged from the top instead oi thebottom. Fluids may be introduced at points midway thetopandbottomoi'theiluidizedmassbesldesat the bottom. Nevertheless, theprocess comprises fluidizing solids in a moving fluid-fluid stream-andcontrolling the nature, amount, velocity and temperature of the fluid.The fluid is preferably gaseous, which may comprise a plurality ofgases, some of which may react with one another under proper temperatureconditions and some of which may react with a portion of the solids. Theselection 01' the gases may be made with the thought oi controllingtemperature in the fluidised mass. I'br example, using coal as the solidmaterial, combustiblegasandoxygenorairmaybeusedalongwithorwithoutsteamorinertsandthequantity of oxygen used may be just thatamount required to maintain the desired temperature of the fluid streamcontacting the solids. Again. an excess of oxygen may be used, \mderwhich condition some of the volatile matter from the coal enters intochemical reaction with it.

Results are obtainable in a fluid through a fluidized mass of solidsthat can not readily be duplicated by the fluids through a stationarybed of the solids. This is particularly true with respect to uniformityof temperature of the surface 0! the. solids, ab-

. is s? ess. attention is called'to the fact instances in which the.process is applies temperatures are desired. :Indrying hood of 275 to400 C. is preferred. lnmaking carbon-black much higher'temperatln-esuallyn.

It probably is obvious thatthe' temperature oithe gas or fluid leavingthe reactim chamber may: be very high. For this reasonchamber ll;FigureLisrei'erredtoasaheatexchangenintending the term to include aboiler which'may', under some conditions, be a preferred type of heatexchanger.

When condensable substanoessuch as benzol, phenol, water or the likeareused as components oi the fluid introduced into the fluidized mass I,Figure 1, chamber It may be used to vaporize them, utilizing theavailable waste heat-sensible heat of the gaseous reaction products. Themeans for separately admitting such substances tollisnotseparatelyshowmBefore stating my specific claims Idesireto call attention to anotherparticular case in which I am able to employ my process andwhich'lbelieve is broadly included in the fluidised solids comprise a suitablecatalyst, such as one containing Ni, Co, or them or other substanceknown to re actions between steam and hydrocarbons, itis possible atrelatively low temperature-below 1000' C.-to produce CO and H2. Thereactions are represented by the following equations:

In certain exothermic reactions where high temperatures favor aparticular reaction the product sought decomposes on prolonged exposureto highly heated surfaces. Such reactions can be conductedadvantageously by my process. The time of contact can be reduced to thewtimum point as determined for a particular case by experiment, byincreasing the velocity of the reactants through the fluidized mass. Anexample of such a reaction is: 2CH4 --C2H2+3Hz. A similar equation canbe written for the production of benzol. In each case low pressure ismore favorable to the reactions. than high pressure. The yields arehigher as the pressure is reduced, but appreciable yields are obtainableunder pressure conditions existing in conducting the process withoutemploying pressure less than atmospheric. However, it should be notedthat reduced pressure can be maintained in the fluidized mass bywithdrawing the products from the confining chamber instead of employingpressure as a fluidizing agent.

I have found that when a prepared catalyst containing or comprising ironis used in I as the suspended medium, it is possible to producecarbon-black of an excellent quality from producer gas, blast-fumacegas, water gas or other gas containing carbon monoxide, by catalyzedchemical reaction represented by the equation, 2CO=CO2+C+ about 71,000B. t. u. which occurs readily at elevated temperatures. ferredtemperature is above 200 C. and below 400 C. The reaction is exothermicand must occur within definite limits because at high tem-' peraturesthe reverse reaction occurs. Also, at about 400 C. iron begins tofunction as a reducing agent for CO2. Cooled gases or steam or both maybe used as a means of temperature control.

In the production of sponge iron a uniform product is obtained when theiron oxide (raw material) is treated suspended in a fluid as described.

I have found that to maintain a mass of solids in suspension in a risingstream of aeriform fluid a definite minimum velocity of fluid isrequired which is a function of several variables. Considering theparticles of solids to be spheres this minimum velocity is expressed bythe mathematical formula, substantially as follows:

where d =density of the aeriform fluid, and

o'=the acceleration due to gravity, in C. G. S.

units.

This relation does not hold exactly for particles of irregular shapewith which somewhat more fluid flow is required. Upon starting, withoutmechanical aid a pressure is created under the perforated plate I whichis equivalent to more than the weight of the mass of solids. For exampleif the weight of a column of the mass having 1 foot sectional area is100 pounds, the pressure necessary to start the operation is greaterthan 100 pounds per square foot. After the particles are fluidized thepressure drops below the initial pressure. Velocities much greater thanlifting-velocity--necessary fluidizing velocity-can be used withsatisfactory results.

The pre-' I However, when there is appreciable difference in the sizesof particles the flner sizes are more readily blown out of chamber l. Ifound, using sand at atmospheric temperature in a bed 18 inches deep,that 50 cubic feet of air per minute per square foot sectional area ofthe mass (area of perforated support) is sufficient to maintain theparticles in a fluidized condition.

When operation is once started it is possible to regulate the flow offluids passing through II by controlling and using the by-pass valveshown at 33 in Fig. l.

Crushed I solids have been referred to throughout the foregoing but theterm is used as inclusive of small particles of the sizes specifiedregardless of how they are made.

Although Figure 2 embodies another-form of apparatus or, rather, amodified form of the apparatus shown in Figure 1, nevertheless, theprocess as practiced therein is considered to be the same as hereindescribed. Referring to Figure 2 the fluidized mass 2, can be made tocirculate automatically by merely opening valves 8A and 8. The fluidizedsolids overflow like a liquid and pass down through BA into chamber IA,as indicated at 2A out of chamber IA through valve 8 and again intochamber I. The flow of fluid through 3 in chamber I is the means bothfor fluidizing and circulating the solids.

The term fluidized mass as used herein and in the claims does not referto a gas containing entrained particles nor to a gas through whichparticles are falling in a shower, such as in the ordinary combustion ofpowdered fuel; it is used to designate a pseudo-fluid such as is formedby passing an aeriform fluid upwardly through a "substantiallystationary mass of confined substantially uniformly sized particles ofsolid material at such a rate that the particles assume limited freedomof motion, the whole having physical properties similar to those of aboiling liquid. The particles are not entrained in the aeriform fluidbut are in vibrant motion and the turbulent motion of a boiling fluid.The pseudoliquid is the fluidized mass having a density much greaterthan that the same aeriform fluid with entrained particles of the samekind of solid. Thus is a "fluidized mass as the term is used herein, thelineal motion of the particles is much less than that of the particlesentrained in a gaseous medium, and likewise, the concentration of theparticles (mass per unit of volume) is greater in the former than in thelatter instance. The fluidized mass" may be produced by the velocityefiect of upwardly blasting an initially stationary bed of solids(preferably uniformly sized solids) with an aeriform fluid at such arate that the particles of. said solids assume limited motion withoutbeing entrained in said fluid; the fluid passing continuously upwardlythrough said mass of solids. This differentiates my fluidized mass fromother forms of suspensions so far as I am aware. The almost obviousbeneflt derived from the employment of the dense, fluidized mass is itsgreater heat capacity per unit of container volume than that ofsuspensions of the same solids entrained in the fluid. If air is blownupwardly through a mass of quicksand under the velocity conditionsdefined above, the mass of sand would be a fluidized mass".

In the appended claims the term gaseous is employed to designate bothsubstances which are gaseous under normal conditions of temperatureupwardly through a confined layer of granular catalytic material ofconsiderable depth at such a rate that said layer is maintained in astate of motion such that the layer presents the appearance of a boilingliquid, meanwhile maintaining the temperature of said material favorablefor causing chemical reaction between said fluids, thereby formingchemical reaction products essentially from said fluids by virtue oftheir intimatecontact with said material, and withdrawing them in saidstream.

2.. A process of producing vapor phase chemical reactions in a gaseousfluid stream, comprising, passing a gaseous stream initially containingtwo gaseous reactants capable of chemically combining with one anotherat elevated temperature upwardly through but in contact with a layer ofconsiderable depth of a substantially granular catalyst at such a ratethat said layer is maintained in a state of motion such that the layerpresents the appearance ofa boiling liquid, meanwhile maintaining saidcatalyst 'at a temperature of 275 to 1000 0., thereby forming chemicalreaction products essentially from said gaseous reactants andwithdrawing them in said stream.

3. A process of producing chemical reactions in a gaseous fluid stream,comprising, passing a stream initially comprised of a gaseoushydrocarbon and steam into contact with and upwardly through a confinedmass of considerable depth of finely divided, solid, incombustiblecontact material, simultaneously maintaining the particles of saidmaterial in a state of ebullient motion substantially by virtue of thevelocity of said stream, causing pyrolysis oi said hydrocarbon in thepresence of said steam by virtue of contact with said material formingcarbon black and a combustible gas, removing the reaction products fromsaid mass in said stream, meanwhile maintaining the temperature of saidmaterial favorable for the pyrolysis of said hydrocarbon. andsubsequently separating said carbon black from said stream.

4. A process of producing chemical reactions in a gaseous fluid stream,comprising, passing a stream initially comprised of a gaseoushydrocarbon and steam into contact with and upwardly through a confinedmass of considerable depth of finely divided, solid, incombustible,contact material, simultaneously maintaining the particles of saidmaterial in a state of ebullient motion substantially by virtue of thevelocity of'said stream, causing pyrolysis of said hydrocarbon in thepresence oi said steam by virtue of contact with said material formingcarbon black and a combustible gas, removing the reaction products fromsaid mass in said stream, and subsequently separately recovering saidcarbon black, and meanwhile maintaining the temperature of said materialfavorable for the pyrolysis of said hydrocarbon, by burning acombustible gas in contact with said material.

5. A process of producing vapor phase chemical reactions in a gaseousfluid-stream, comprising, passing a stream initially comprised of agaseous hydrocarbon and a gaseous oxidizing agent into contact with andupwardly through a confined mass of considerable depth of finelydivided,

solid, incombustible, catalytic contact material, simultaneouslymaintaining the particles of said material in a state of ebullientmotion substantially by virtue of the velocity of said stream, causingsaid hydrocarbon and said oxidizing agent to react chemically with oneanother by virtue of the catalytic efl'ect oi said material forming acombustible gas and removing said gas from said mass in said stream, andmeanwhile maintaining the temperature of said material favorable for thegeneration of said gas.

6. In the process defined in claim 5, heating said mass by introducingboth air and ignited combustible gas into said mass.

7. In the process defined in claim 5, maintaining the temperature ofsaid material by burning sufllcient combustible gas with air in contactwith said material simultaneous with the passage therethrough of saidhydrocarbon.

8. A process of producing vapor phase chemical reactions in a gaseousfluid-stream, comprising, passing said gaseous stream into contact withand upwardly through a confined layer of granular catalytic materialunreactive with the said gaseous stream and of substantially uniiormlysized particles and of considerable depth at such a rate that said layeris maintained in a state 01' motion such that the layer presents theappearance of a boiling liquid, meanwhile, maintaining the temperatureof said material favorable for causing said gaseous fluid to undergoreaction thereby forming reaction products essentially from said fluidby virtue oi its intimate contact with said material, and withdrawingthem in said stream.

9. A process of producing vapor phase chemical reactions in a gaseousfluid stream, comprising, passing a gaseous stream at elevatedtemperature upwardly through but in contact with a layer of considerabledepth of a catalyst bed of substantially uniformly sized particlesunreactive with the said gaseous stream at such a rate that said layeris maintained in a state of motion such that the layer presents theappearance of a boiling liquid, meanwhile maintaining said catalyst at atemperature of 275 to 1000 0., thereby forming chemical reactionproducts essentially from said gases and withdrawing them in saidstream.

10. A process for producing a chemical reaction in a gasiform streamwhich comprises passing a gasiform stream containing a gasiformthermally-convertible hydrocarbon material upwardly through a bed ofgranular particles of substantially uniform size oi solid incombustiblecatalytic material at a speed suflicient to maintain said particles inebullient motion and to thereby impart to said mass of particles theappearance of a bofling liquid but insufilcient to carry away anysubstantial proportion of said particles from the main body of saidmass, maintaining said mass at a temperature suitable for the desiredchemical reaction and withdrawing reaction products from said mass insaid stream substantially as they are formed.

11. A process of producing chemical reactions in a gaseous fluid streamcomprising passing a gasiform stream comprised of at least a gasiformhydrocarbon into contact with and upwardly through a confined mass ofconsiderable depth of finely divided solid incombustible catalyticcontact material simultaneously maintaining the particles of saidmaterial in a state of ebullient motion substantially by virtue of thevelocity of said stream, causing Pyrolysis of said hydrocarcontactmaterial, simultaneously maintaining the particles of said material in astate of ebullient motion substantially by virtue of the velocity ofsaid stream, causing cracking of said hydrocarbon by virtue of contactwith said catalytic material, removing the reaction products from saidmass in said stream, meanwhile maintaining the temperature of saidmaterial favorable for the cracking of said hydrocarbon and subsequentlyseparating the reaction products from said 10 stream.

WILLIAM W. ODELL.

